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Two-dimensional (2D) transition metal dichalcogenide (TMDC) materials have garnered great attention on account of their novel properties and potential to advance modern technology. Recent studies have demonstrated that TMDCs can be utilized to create high-performing heterostructures with combined functionality of the individual layers and new phenomena at these interfaces. Here, we report an ultrafast photoresponse within MoSe2-based heterostructures in which heavily p-doped WSe2 and MoS2 flakes share an undoped MoSe2 channel, allowing us to directly compare the optoelectronic properties of MoSe2-based heterojunctions with different 2D materials. Strong photocurrent signals have been observed in both MoSe2−WSe2 and MoSe2−MoS2 heterojunctions with a photoresponse time constant of ∼16 μs, surmounting previous MoSe2-based devices by three orders of magnitude. Further studies have shown that the fast response is independent of the integrated 2D materials (WSe2 or MoS2) but is likely attributed to the high carrier mobility of 260 cm V−1 s−1 in the undoped MoSe2 channel as well as the greatly reduced Schottky barriers and near absence of interface states at MoSe2−WSe2/MoS2 heterojunctions, which lead to reduced carrier transit time and thus short photocurrent response time. Lastly, a high detectivity on the order of ∼10 Jones has been achieved in MoSe2-based heterojunctions, which supersedes current industry standards. These fundamental studies not only shed light on photocurrent generation mechanisms in MoSe2-based heterojunctions but also open up new avenues for engineering future high-performance 2D optoelectronic devices.

Ultrafast Photocurrent Response and High Detectivity in Two-Dimensional MoSe2-based Heterojunctions